Your browser doesn't support javascript.
loading
: 20 | 50 | 100
1 - 20 de 30
1.
ACS Nano ; 18(24): 15681-15694, 2024 Jun 18.
Article En | MEDLINE | ID: mdl-38848285

The prolonged wound-healing process caused by pathogen infection remains a major public health challenge. The developed electrical antibiotic administration typically requires metal electrodes wired to a continuous power supply, restricting their use beyond clinical environments. To obviate the necessity for antibiotics and an external power source, we have developed a wearable synergistic electroceutical device composed of an air self-charging Zn battery. This battery integrates sustained tissue regeneration and antibacterial modalities while maintaining more than half of the initial capacity after ten cycles of chemical charging. In vitro bacterial/cell coculture with the self-charging battery demonstrates inhibited bacterial activity and enhanced cell function by simulating the endogenous electric field and dynamically engineering the microenvironment with released chemicals. This electroceutical device provides accelerated healing of a bacteria-infected wound by stimulating angiogenesis and modulating inflammation, while effectively inhibiting bacterial growth at the wound site. Considering the simple structure and easy operation for long-term treatment, this self-charging electroceutical device offers great potential for personalized wound care.


Anti-Bacterial Agents , Wearable Electronic Devices , Wound Healing , Animals , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemistry , Humans , Mice , Staphylococcus aureus/physiology , Zinc/chemistry , Escherichia coli , Microbial Sensitivity Tests
2.
J Colloid Interface Sci ; 669: 835-843, 2024 Sep.
Article En | MEDLINE | ID: mdl-38749222

Wearable drug delivery systems (DDS) have made significant advancements in the field of precision medicine, offering precise regulation of drug dosage, location, and timing. The performance qualities that wearable DDS has always strived for are simplicity, efficiency, and intelligence. This paper proposes a wearable dual-drug synergistic release patch. The patch is powered by a built-in magnesium battery and utilizes a hydrogel containing viologen-based hyperbranched polyamidoamine as both a cathode material and an integrated drug reservoir. This design allows for the simultaneous release of both dexamethasone and tannic acid, overcoming the limitations of monotherapy and ensuring effective synergy for on-demand therapy. In a mouse model with praziquimod-induced psoriasis, the patch demonstrated therapeutic efficacy at a low voltage. The inflammatory skin returned to normal after 5 days with the on-demand release of dual drugs. This work provides a promising treatment option considering its straightforward construction and the therapeutic advantages of dual-drug synergy.


Dexamethasone , Psoriasis , Wearable Electronic Devices , Animals , Mice , Psoriasis/drug therapy , Psoriasis/pathology , Dexamethasone/administration & dosage , Dexamethasone/pharmacology , Delayed-Action Preparations/chemistry , Tannins/chemistry , Tannins/pharmacology , Drug Liberation , Hydrogels/chemistry , Drug Delivery Systems , Transdermal Patch , Polyamines
3.
Front Immunol ; 15: 1366096, 2024.
Article En | MEDLINE | ID: mdl-38596689

Background: The tumor microenvironment (TME) plays a pivotal role in the progression and metastasis of lung adenocarcinoma (LUAD). However, the detailed characteristics of LUAD and its associated microenvironment are yet to be extensively explored. This study aims to delineate a comprehensive profile of the immune cells within the LUAD microenvironment, including CD8+ T cells, CD4+ T cells, and myeloid cells. Subsequently, based on marker genes of exhausted CD8+ T cells, we aim to establish a prognostic model for LUAD. Method: Utilizing the Seurat and Scanpy packages, we successfully constructed an immune microenvironment atlas for LUAD. The Monocle3 and PAGA algorithms were employed for pseudotime analysis, pySCENIC for transcription factor analysis, and CellChat for analyzing intercellular communication. Following this, a prognostic model for LUAD was developed, based on the marker genes of exhausted CD8+ T cells, enabling effective risk stratification in LUAD patients. Our study included a thorough analysis to identify differences in TME, mutation landscape, and enrichment across varying risk groups. Moreover, by integrating risk scores with clinical features, we developed a new nomogram. The expression of model genes was validated via RT-PCR, and a series of cellular experiments were conducted, elucidating the potential oncogenic mechanisms of GALNT2. Results: Our study developed a single-cell atlas for LUAD from scRNA-seq data of 19 patients, examining crucial immune cells in LUAD's microenvironment. We underscored pDCs' role in antigen processing and established a Cox regression model based on CD8_Tex-LAYN genes for risk assessment. Additionally, we contrasted prognosis and tumor environments across risk groups, constructed a new nomogram integrating clinical features, validated the expression of model genes via RT-PCR, and confirmed GALNT2's function in LUAD through cellular experiments, thereby enhancing our understanding and approach to LUAD treatment. Conclusion: The creation of a LUAD single-cell atlas in our study offered new insights into its tumor microenvironment and immune cell interactions, highlighting the importance of key genes associated with exhausted CD8+ T cells. These discoveries have enabled the development of an effective prognostic model for LUAD and identified GALNT2 as a potential therapeutic target, significantly contributing to the improvement of LUAD diagnosis and treatment strategies.


Adenocarcinoma of Lung , Lung Neoplasms , Humans , Prognosis , CD8-Positive T-Lymphocytes , Nomograms , Lung Neoplasms/genetics , Tumor Microenvironment , Lectins, C-Type
4.
Angew Chem Int Ed Engl ; 63(18): e202401629, 2024 Apr 24.
Article En | MEDLINE | ID: mdl-38385954

Aqueous zinc-ion batteries (ZIBs) are safe and economical for grid applications. However, current ZIBs have limitations in terms of inferior capacity and low output voltage, which are hampered by the electrolyte applicability of the Zn2+ hosts. In this study, we propose a novel organic cathode design strategy with a bifunctional potential region. This polymeric Zn2+ host combines the conjugated polyaniline backbone to tune the molecular surface pH and [Fe(CN)6]3-/4- redox couple for high output voltage and capacity. The polyaniline doped with ferricyanide (PAF) electrode exhibits two forms of charge storage in ZIBs: proton-assisted Zn2+ doping below 1.2 V (mechanism I), and [Fe(CN)6]3-/4- redox pair above 1.8 V (mechanism II). Density functional theory calculations and in situ pH experiments demonstrated that the H+ doping process of mechanism I forms a localized pH regulation on the molecular chain surface, providing a favorable reaction environment for mechanism II. The Zn-polymer battery delivered an outstanding discharge capacity (405.2 mAh g-1) and high output voltage (1.8 V) in the Zn(CF3SO3)2 electrolyte. This study provides a new route for enhancing the structural stability of electrodes and overcoming the electrolyte limitations of ferricyanide in weakly acidic electrolytes.

5.
Cancer Imaging ; 23(1): 83, 2023 Sep 07.
Article En | MEDLINE | ID: mdl-37679806

OBJECTIVE: To develop and validate a prediction model for early recurrence of stage I lung adenocarcinoma (LUAD) that combines radiomics features based on preoperative CT with tumour spread through air spaces (STAS). MATERIALS AND METHODS: The most recent preoperative thin-section chest CT scans and postoperative pathological haematoxylin and eosin-stained sections were retrospectively collected from patients with a postoperative pathological diagnosis of stage I LUAD. Regions of interest were manually segmented, and radiomics features were extracted from the tumour and peritumoral regions extended by 3 voxel units, 6 voxel units, and 12 voxel units, and 2D and 3D deep learning image features were extracted by convolutional neural networks. Then, the RAdiomics Integrated with STAS model (RAISm) was constructed. The performance of RAISm was then evaluated in a development cohort and validation cohort. RESULTS: A total of 226 patients from two medical centres from January 2015 to December 2018 were retrospectively included as the development cohort for the model and were randomly split into a training set (72.6%, n = 164) and a test set (27.4%, n = 62). From June 2019 to December 2019, 51 patients were included in the validation cohort. RAISm had excellent discrimination in predicting the early recurrence of stage I LUAD in the training cohort (AUC = 0.847, 95% CI 0.762-0.932) and validation cohort (AUC = 0.817, 95% CI 0.625-1.000). RAISm outperformed single modality signatures and other combinations of signatures in terms of discrimination and clinical net benefits. CONCLUSION: We pioneered combining preoperative CT-based radiomics with STAS to predict stage I LUAD recurrence postoperatively and confirmed the superior effect of the model in validation cohorts, showing its potential to assist in postoperative treatment strategies.


Adenocarcinoma of Lung , Lung Neoplasms , Humans , Retrospective Studies , Adenocarcinoma of Lung/diagnostic imaging , Adenocarcinoma of Lung/surgery , Eosine Yellowish-(YS) , Tomography, X-Ray Computed , Lung Neoplasms/diagnostic imaging , Lung Neoplasms/surgery
6.
ACS Appl Mater Interfaces ; 15(32): 38821-38832, 2023 Aug 16.
Article En | MEDLINE | ID: mdl-37540805

The emergence of precision medicine and personalized pharmacotherapy has led to the development of advanced drug delivery systems that can respond to multiple stimuli. Conductive hydrogels have excellent electrical signal responsiveness and drug storage capabilities; however, current conductive hydrogels suffer from poor mechanical properties, low ionic conductivity, and high voltage. Herein, a covalently crosslinked viologen hydrogel was prepared using electroactive hyperbranched polyamidoamine (EHP) as the crosslinking center in a polymeric network. Attributed to its unique molecular architecture, this hydrogel exhibits improved mechanical properties (high tensile strength and desirable stretchability up to 1280%). Approvable ionic conductivity, biocompatibility, antibacterial properties, and wearable strain-sensing performance were also disclosed, ascribed to the participation of versatile viologen groups in the hydrogel structure. This hydrogel exhibited high efficiency in drug release (81.6%) at a lower voltage of -1.2 V. Moreover, fascinating pH-stimulus drug release behavior was also demonstrated in both acidic and alkalescent environments owing to the dramatic conformational transition of EHP. This work provides a new design strategy for conductive hydrogels for multiple stimulus-responsive drug delivery systems.


Drug Delivery Systems , Hydrogels , Hydrogels/pharmacology , Electric Conductivity , Polyamines
7.
Aging (Albany NY) ; 15(14): 6774-6797, 2023 07 11.
Article En | MEDLINE | ID: mdl-37437244

Cancer-associated fibroblasts (CAFs) are an important component of the tumor microenvironment (TME). CAFs can promote tumor occurrence and metastasis by promoting cancer cell proliferation, angiogenesis, extracellular matrix (ECM) remodeling, and drug resistance. Nevertheless, how CAFs are related to Lung adenocarcinoma (LUAD) has not yet been revealed, especially since the CAFs-related prediction model has yet to be established. We combined Single-cell RNA-sequencing (scRNA-seq) and Bulk-RNA data to develop a predictive model of 8 CAFs-associated genes. Our model predicted LUAD prognosis and immunotherapy efficacy. TME, mutation landscape and drug sensitivity differences were also systematically analyzed between the LUAD patients of high- and low-risk. Moreover, the model prognostic performance was validated in four independent validation cohorts in the Gene expression omnibus (GEO) and the IMvigor210 immunotherapy cohort.


Adenocarcinoma of Lung , Cancer-Associated Fibroblasts , Lung Neoplasms , Humans , Prognosis , Adenocarcinoma of Lung/genetics , RNA , Tumor Microenvironment/genetics , Lung Neoplasms/genetics , Single-Cell Analysis
8.
Small ; 19(34): e2301886, 2023 Aug.
Article En | MEDLINE | ID: mdl-37086144

Electrochromic (EC) reflective displays offer great advantages in delivering information and providing visual data, but are limited in dark environments. Reflective/emissive dual-modal displays capable of electrochemically-induced color and fluorescence change simultaneously are highly desirable, especially possessing rapid response speed as well as long-term durability. Herein, an electroactive fluorescent ionic liquid based on triphenylamine and imidazole (EFIL-TPA) has been synthesized for reflective/emissive dual-modal display. The resultant device exhibits outstanding electrochromic/electrofluorochromic (EC/EFC) performance with low driving voltage (below 1.0 V), fast switching speed (0.57-1.8 s), and remarkable cycling durability (91% retention for 10 000 cycles). A piezoelectric nanogenerator (PENG) driven EC/EFC integrated system is fabricated to harvest energy from human motion and visually drive the color/fluorescence change for human motion indication in both bright and dark environments. This innovative EC/EFC dual-modal display device based on EFIL-TPA supports a huge space for the development of self-powered human motion visualized indication in all-light conditions.

9.
Chem Sci ; 14(8): 2123-2130, 2023 Feb 22.
Article En | MEDLINE | ID: mdl-36845924

Implanted rechargeable batteries that can provide energy over a sufficient lifetime and ultimately degrade into non-toxic byproducts are highly desirable. However, their advancement is significantly impeded by the limited toolbox of electrode materials with a known biodegradation profile and high cycling stability. Here we report biocompatible, erodible poly(3,4-ethylenedioxythiophene) (PEDOT) grafted with hydrolyzable carboxylic acid pendants. This molecular arrangement combines the pseudocapacitive charge storage from the conjugated backbones and dissolution via hydrolyzable side chains. It demonstrates complete erosion under aqueous conditions in a pH-dependent manner with a predetermined lifetime. The compact rechargeable Zn battery with a gel electrolyte offers a specific capacity of 31.8 mA h g-1 (57% of theoretical capacity) and outstanding cycling stability (78% capacity retention over 4000 cycles at 0.5 A g-1). Subcutaneous implantation of this Zn battery into Sprague-Dawley (SD) rats demonstrates complete biodegradation in vivo and biocompatibility. This molecular engineering strategy presents a viable avenue for developing implantable conducting polymers with a predetermined degradation profile and high energy storage capability.

10.
Theranostics ; 13(1): 95-105, 2023.
Article En | MEDLINE | ID: mdl-36593956

Background: Lipid droplets (LDs) are critical organelles associated with many physiological processes in eukaryotic cells. To visualize and study LDs, fluorescence imaging techniques including the confocal imaging as well as the emerging super-resolution imaging of stimulated emission depletion (STED), have been regarded as the most useful methods. However, directly limited by the availability of advanced LDs fluorescent probes, the performances of LDs fluorescence imaging are increasingly unsatisfied with respect to the fast research progress of LDs. Methods: We herein newly developed a superior LDs fluorescent probe named Lipi-QA as a powerful tool for LDs fluorescence imaging and biological study. Colocalization imaging of Lipi-QA and LDs fluorescent probe Ph-Red was conducted in four cell lines. The LDs staining selectivity and the photostability of Lipi-QA were also evaluated by comparing with the commercial LDs probe Nile Red. The in-situ fluorescence lifetime of Lipi-QA in LDs was determined by time-gated detection. The cytotoxicity of Lipi-QA was assessed by MTT assay. The STED saturation intensity as well as the power- and gate time-dependent resolution were tested by Leica SP8 STED super-resolution nanoscopy. The time-lapse 3D confocal imaging and time-lapse STED super-resolution imaging were then designed to study the complex physiological functions of LDs. Results: Featuring with the advantages of the super-photostability, high LDs selectivity, long fluorescence lifetime and low STED saturation intensity, the fluorescent probe Lipi-QA was capable of the long-term time-lapse three-dimensional (3D) confocal imaging to in-situ monitor LDs in 3D space and the time-lapse STED super-resolution imaging (up to 500 STED frames) to track the dynamics of LDs with nanoscale resolution (37 nm). Conclusions: Based on the state-of-the-art fluorescence imaging results, some new biological insights into LDs have been successfully provided. For instance, the long-term time-lapse 3D confocal imaging has surely answered an important and controversial question that the number of LDs would significantly decrease rather than increase upon starvation stimulation; the time-lapse STED super-resolution imaging with the highest resolution has impressively uncovered the fission process of nanoscale LDs for the first time; the starvation-induced change of LDs in size and in speed has been further revealed at nanoscale by the STED super-resolution imaging. All of these results not only highlight the utility of the newly developed fluorescent probe but also significantly promote the biological study of LDs.


Fluorescent Dyes , Molecular Probes , Molecular Probes/metabolism , Microscopy, Fluorescence/methods , Fluorescent Dyes/metabolism , Lipid Droplets/metabolism , Optical Imaging
11.
Nat Commun ; 14(1): 297, 2023 01 18.
Article En | MEDLINE | ID: mdl-36653362

Wearable transdermal iontophoresis eliminating the need for external power sources offers advantages for patient-comfort when deploying epidermal diseases treatments. However, current self-powered iontophoresis based on energy harvesters is limited to support efficient therapeutic administration over the long-term operation, owing to the low and inconsistent energy supply. Here we propose a simplified wearable iontophoresis patch with a built-in Mg battery for efficient and controllable transdermal delivery. This system decreases the system complexity and form factors by using viologen-based hydrogels as an integrated drug reservoir and cathode material, eliminating the conventional interface impedance between the electrode and drug reservoir. The redox-active polyelectrolyte hydrogel offers a high energy density of 3.57 mWh cm-2, and an optimal bioelectronic interface with ultra-soft nature and low tissue-interface impedance. The delivery dosage can be readily manipulated by tuning the viologen hydrogel and the iontophoresis stimulation mode. This iontophoresis patch demonstrates an effective treatment of an imiquimod-induced psoriasis mouse. Considering the advantages of being a reliable and efficient energy supply, simplified configuration, and optimal electrical skin-device interface, this battery-powered iontophoresis may provide a new non-invasive treatment for chronic epidermal diseases.


Iontophoresis , Skin , Mice , Animals , Administration, Cutaneous , Skin/metabolism , Skin Absorption , Hydrogels/metabolism , Drug Delivery Systems
12.
Nanomicro Lett ; 14(1): 219, 2022 Nov 10.
Article En | MEDLINE | ID: mdl-36355311

Metallic interface engineering is a promising strategy to stabilize Zn anode via promoting Zn2+ uniform deposition. However, strong interactions between the coating and Zn2+ and sluggish transport of Zn2+ lead to high anodic polarization. Here, we present a bio-inspired silk fibroin (SF) coating with amphoteric charges to construct an interface reversible electric field, which manipulates the transfer kinetics of Zn2+ and reduces anodic polarization. The alternating positively and negatively charged surface as a build-in driving force can expedite and homogenize Zn2+ flux via the interplay between the charged coating and adsorbed ions, endowing the Zn-SF anode with low polarization voltage and stable plating/stripping. Experimental analyses with theoretical calculations suggest that SF can facilitate the desolvation of [Zn(H2O)6]2+ and provide nucleation sites for uniform deposition. Consequently, the Zn-SF anode delivers a high-rate performance with low voltage polarization (83 mV at 20 mA cm-2) and excellent stability (1500 h at 1 mA cm-2; 500 h at 10 mA cm-2), realizing exceptional cumulative capacity of 2.5 Ah cm-2. The full cell coupled with ZnxV2O5·nH2O (ZnVO) cathode achieves specific energy of ~ 270.5/150.6 Wh kg-1 (at 0.5/10 A g-1) with ~ 99.8% Coulombic efficiency and retains ~ 80.3% (at 5.0 A g-1) after 3000 cycles.

13.
Macromol Rapid Commun ; 43(20): e2200347, 2022 Oct.
Article En | MEDLINE | ID: mdl-35686689

Yarn supercapacitors have attracted significant attention for wearable energy storage due to their ability to be directly integrated with garments. Conducting polymer polypyrrole (PPy) based yarn supercapacitors show limited cycling stability because of the huge volume changes during the charge-discharge processes. In addition, laundering may cause damage to such yarn supercapacitors. Here, the fabrication of PPy-based re-stickable yarn supercapacitors is reported with good cycling stability by employing vapor phase polymerization (VPP) and water-soluble polyethylene oxide (PEO) film as the adhesive layer. VPP duration and cycle are controlled to achieve multi-layered PPy electrodes. The assembled yarn supercapacitors show a good cycling stability with capacitance retention of 79.1% after 5000 charge-discharge cycles. The energy stored in the yarn supercapacitor is sufficient to power a photodetector. After gluing the yarn supercapacitors onto a PEO film, the devices can be stunk on and peeled off the garment to avoid the mechanical stresses during the washing process. Three yarn supercapacitors connected in parallel on PEO film show negative changes in electrochemical performance after 5 sticking-peeling cycles. This work provides a facile way to fabricate PPy-based re-stickable energy storage devices with high cycling stability for smart garments.

14.
Small Methods ; 6(7): e2200344, 2022 07.
Article En | MEDLINE | ID: mdl-35689331

Iron is a promising material for cardiovascular stent applications, however, the low biodegradation rate presents a challenge. Here, a dynamic method to improve the degradation rate of iron and simultaneously deliver electrical energy that could potentially inhibit cell proliferation on the device is reported. It is realized by pairing iron with a biocompatible hydrogel cathode in a cell culture media-based electrolyte forming an iron-air battery. This system does not show cytotoxicity to human adipose-stem cells over a period of 21 days but inhibits cell proliferation. The combination of enhanced iron degradation and inhibited cell proliferation by this dynamic method suggests it might be an approach for restenosis inhibition of biodegradable stents.


Iron , Stents , Humans , Iron/pharmacology
15.
Anal Chem ; 94(16): 6271-6280, 2022 04 26.
Article En | MEDLINE | ID: mdl-35417142

Modulating the precise self-assembly of functional biomacromolecules is a critical challenge in biotechnology. Herein, functional biomacromolecule-assembled hierarchical hybrid nanoarchitectures in a spatially controlled fashion are synthesized, achieving the biorecognition behavior and signal amplification in the immunoassay simultaneously. Biomacromolecules with sequential assembly on the scaffold through the biomineralization process show significantly enhanced stability, bioactivity, and utilization efficiency, allowing tuning of their functions by modifying their size and composition. The hierarchically hybrid nanoarchitectures show great potential in construction of ultrasensitive immunoassay platforms, achieving a three order-of-magnitude increase in sensitivity. Notably, the well-designed HRP@Ab2 nanoarchitectures allow for optical immunoassays with a detection range from picogram mL-1 to microgram mL-1 on demand, providing great promise for quantitative analysis of both low-abundance and high-residue targets for biomedical applications.


Immunologic Tests , Proteins , Immunoassay
16.
Biosens Bioelectron ; 206: 114132, 2022 Jun 15.
Article En | MEDLINE | ID: mdl-35245869

Fundamentally improving the sensing sensitivity of immunoassay remains a huge challenge, which limited further critical applications. Herein we designed a new immunoprobe by integrating biometric unit (antibody) and signal amplification element (enzyme) to form urease-antibody-CaHPO4 hybrid nanoflower (UAhNF) via the biomineralization process. The dual-functional UAhNF enhances the stability of urease in NaCl (10 mmol L-1) and high temperature (60 °C), and also maintains the ability of antibody recognition, fitting greatly well with the need for immunosensor. Using imidacloprid as a model target, the fixed coating antigens are competed with imidacloprid to capture primary antibodies, and the secondary antibody of UAhNF was linked to construct the competitive-type fluorogenic immunoassays. An in-situ etching process of copper nanoparticles initiated by urease is integrated with UAhNF-based immune response for further improving the detection sensitivity. The proposed immunosensor possessed a 50% inhibition concentration value of 0.72 ng mL-1, which is 30-fold lower than conventional enzyme-linked immunosorbent assay. This presented approach provided a versatile sensing tool by varying building blocks, making it practically functional for a variety of bioassay applications.


Biosensing Techniques , Nanostructures , Antibodies , Enzyme-Linked Immunosorbent Assay , Gold , Immunoassay , Nanostructures/chemistry , Urease
17.
Nanomicro Lett ; 14(1): 56, 2022 Feb 05.
Article En | MEDLINE | ID: mdl-35122157

Environmentally friendly degradable sensors with both hazardous gases and pressure efficient sensing capabilities are highly desired for various promising applications, including environmental pollution monitoring/prevention, wisdom medical, wearable smart devices, and artificial intelligence. However, the transient gas and pressure sensors based on only identical sensing material that concurrently meets the above detection needs have not been reported. Here, we present transient all-MXene NO2 and pressure sensors employing three-dimensional porous crumpled MXene spheres prepared by ultrasonic spray pyrolysis technology as the sensing layer, accompanied with water-soluble polyvinyl alcohol substrates embedded with patterned MXene electrodes. The gas sensor achieves a ppb-level of highly selective NO2 sensing, with a response of up to 12.11% at 5 ppm NO2 and a detection range of 50 ppb-5 ppm, while the pressure sensor has an extremely wide linear pressure detection range of 0.14-22.22 kPa and fast response time of 34 ms. In parallel, all-MXene NO2 and pressure sensors can be rapidly degraded in medical H2O2 within 6 h. This work provides a new avenue toward environmental monitoring, human physiological signal monitoring, and recyclable transient electronics.

18.
ACS Appl Mater Interfaces ; 14(1): 428-438, 2022 Jan 12.
Article En | MEDLINE | ID: mdl-34964605

Cholesterol is a vital compound in maintenance for human health, and its concentration levels are tightly associated with various diseases. Therefore, accurate monitoring of cholesterol is of great significance in clinical diagnosis. Herein, we fabricated a noncontact biosensor based on photonic crystal-enhanced upconversion nanoparticles (UCNPs) for highly sensitive and interference-free cholesterol detection. By compounding LiErF4:0.5%Tm3+@LiYF4 UCNPs with poly(methyl methacrylate) (PMMA) photonic crystals (OPCs), we were able to selectively tune the coupling of the photonic band gap to the excitation field and modulate the upconversion (UC) luminescence intensity, given the unique multi-wavelength excitation property of LiErF4:0.5%Tm3+@LiYF4. A 48.5-fold enhancement of the monochromatic red UC emission was ultimately achieved at 980 nm excitation, ensuring improved detection sensitivity. Based on the principle of quenching of the intense monochromic red UC emission by the oxidation products of 3,3',5,5'-tetramethylbenzidine (TMB) yielded from the cholesterol cascade reactions, the biosensor has a detection limit of 1.6 µM for cholesterol with excellent specificity and stability. In addition, the testing results of the as-designed biosensor in patients are highly consistent with clinical diagnostic data, providing a sensitive, reliable, reusable, interference-free, and alternative strategy for clinical cholesterol detection.


Biocompatible Materials/chemistry , Biosensing Techniques , Cholesterol/blood , Nanoparticles/analysis , Photons , Erbium/chemistry , Fluorine/chemistry , Humans , Lithium/chemistry , Materials Testing , Particle Size , Thulium/chemistry , Yttrium/chemistry
19.
Environ Res ; 203: 111844, 2022 01.
Article En | MEDLINE | ID: mdl-34364861

This work for the first time reports bimetallic Ni-Co and monometallic (Ni and Co) nanoparticles (NPs)-engineered carbon nitride nanotubes with nitrogen vacancies (V-CNNTs) for visible-light photocatalytic H2 generation application. The bimetallic Ni-Co NPs have an average size of less than 5 nm and are homogenously dispersed along the nanochannels of V-CNNTs. The composition of the bimetallic NPs plays an essential role to maximize photocatalytic activity. With the optimal Ni/Co atom ratio of 3:1, Ni-Co/V-CNNTs nanohybrids yielded a H2 production rate of 4.19 µmol/h, which is higher than those of monometallic counterparts and V-CNNTs. The intimately loaded Ni-Co NPs and incorporated nitrogen vacancies enhance the photocatalytic performance through extended light absorption, abundant active sites, strong metal-support interaction, and efficient charge carrier transfer along the axial direction. This study presents a stable and highly efficient hybrid as a promising photocatalyst for visible light photocatalytic H2 production through water splitting.


Nanoparticles , Nanotubes , Catalysis , Hydrogen , Nitriles , Nitrogen
20.
Adv Sci (Weinh) ; 9(4): e2103896, 2022 02.
Article En | MEDLINE | ID: mdl-34914857

Aqueous all-polymer proton batteries (APPBs) consisting of redox-active polymer electrodes are considered safe and clean renewable energy storage sources. However, there remain formidable challenges for APPBs to withstand a high current rate while maximizing high cell output voltage within a narrow electrochemical window of aqueous electrolytes. Here, a capacitive-type polymer cathode material is designed by grafting poly(3,4-ethylenedioxythiophene) (PEDOT) with bioinspired redox-active catechol pendants, which delivers high redox potential (0.60 V vs Ag/AgCl) and remarkable rate capability. The pseudocapacitive-dominated proton storage mechanism illustrated by the density functional theory (DFT) calculation and electrochemical kinetics analysis is favorable for delivering fast charge/discharge rates. Coupled with a diffusion-type anthraquinone-based polymer anode, the APPB offers a high cell voltage of 0.72 V, outstanding rate capability (64.8% capacity retention from 0.5 to 25 A g-1 ), and cycling stability (80% capacity retention over 1000 cycles at 2 A g-1 ), which is superior to the state-of-the-art all-organic proton batteries. This strategy and insight provided by DFT and ex situ characterizations offer a new perspective on the delicate design of polymer electrode patterns for high-performance APPBs.

...